Building a consistent and reproducible database for adsorption evaluation in Covalent-Organic Frameworks

We present a workflow that traces the path from the bulk structure of a crystalline material to assessing its performance in carbon capture from coal's post-combustion flue gases. We apply the workflow to a database of 324 covalent-organic frameworks (COFs) reported in the literature to characterize their CO2 adsorption properties using the following steps: (1) optimization of the crystal structure (atomic positions and cell) using density functional theory, (2) fitting atomic point charges based on the electron density, (3) characterizing the (pore) geometry of the structures before and after optimization, (4) computing carbon dioxide and nitrogen isotherms using grand canonical Monte Carlo simulations (empirical interaction potential) and, finally, (5) assessing the CO2 parasitic energy via process modelling. The full workflow has been encoded in the Automated Interactive Infrastructure and Database for Computational Science (AiiDA). Both the workflow and the automatically generated provenance graph of our calculations are made available on the Materials Cloud, allowing peers to inspect inspect every input parameter and result along the workflow, download structures and files at intermediate stages and start their research right from where this work has left off. In particular, our set of CURATED COFs with optimized geometry and high quality DFT-derived point charges is available for further investigations of gas adsorption properties. We plan to update the database as new COFs are being reported.